Enriched aqueous components of emblica officinalis

ABSTRACT

In an extraction process comprising extracting a raw extract from  Emblica officinalis  the improvement comprising conducting the extraction under conditions of time, temperature and atmosphere, to inhibit the formation of black specks and/or oligomeric and/or polymeric tannins and/or oxidation products thereof.

This invention relates to methods of eliminating undesired substances,including but not limited to oligomeric/polymeric components fromcompositions obtained from the fruit of Emblica officinalis plant alsoknown as Phyllanthus Emblica and the resulting enriched compositions.This plant is generally found in India, China, Pakistan, Nepal and othercountries. Accordingly, this invention is directed to extracts ofEmblica officinalis from any geographical location.

Compositions obtained from an extract of the fruit of the Emblicaofficinalis plant have been described in the prior art, for example, inthe above cross-referenced allowed application Ser. No. 10/120,156, thereferences referred to therein, as well as in U.S. Pat. No. 6,235,721issued May 22, 2001 and U.S. Pat. No. 6,636,162 issued Mar. 26, 2002.

In U.S. Pat. No. 6,235,721, an anti-oxidant product referred to as“CAPROS” is isolated from the fruit of Emblica officinalis plant using avery dilute aqueous or alcoholic water salt solution, e.g. a 0.1 to 5%(w/w), preferably 1 to 2%, of a sodium chloride, potassium chloride,calcium chloride or magnesium chloride solution, which preventsdegradation of the anti-oxidant compounds therein by enzymes present inthe fruits of the Emblica officinalis plant. Alternatively, theanti-oxidant product is isolated using a buffer solution, e.g. 0.1 to 5%(w/w), preferably 1 to 2%, of sodium citrate/citric acid, sodiumacetate/acetic acid, sodium phosphate/phosphoric acid, instead ofaqueous or alcoholic water salt solution. It is further stated in thispatent that the composition contains, by weight, Embilcanin-A and B(gallic/ellagic acid derivatives of 2-keto-glucono-δ-lactone) (35-55%),Punigluconin (2,3-di-O-galloyl-0,6-(S)-hexahydroxy-diphenoylgluconicacid) 4-15%), Pedunculagin(2,3,4,6-bis-(S)-hexahydroxydiphenoyl-D-glucose) (10-20%); Rutin(flavanol-3-)glycoside (5-15%); low to medium molecular weightgallo-ellagi tannoids (10-30%); gallic acid (0-5%) and ellagic acid(0-5%).

In the application U.S. Ser. No. 10/120,156, a standardized compositionis described which is useful, for example, in skin lightening or skinwhitening. This composition, hereinafter, termed “EMBLICA” isdistinguished from “CAPROS”, by, for example, having less than 1% byweight of total flavonoids and even lower contents of RUTIN. Whereas,light colored EMBLICA consists essentially of the desired components forthe purposes of skin lightening or skin whitening, it has been observedthat black specks in the commercial product diminish the estheticappearance of the final formulations. Other commercially availableproducts based on extracts of Emblica officinalis are even darker incolor due, on information and belief, to the presence of a larger numberof black specks and water-insoluble oligomeric/polymeric materials.

Accordingly, one aspect of this invention is to provide at least oneprocess for the removal of black specks in all types of extracts ofEmblica officinalis so that the resulting composition is macroscopically(visually) devoid of such specks.

Another aspect of this invention is to provide a material substantiallydevoid of water-insoluble oligomeric/polymeric components.

We have discovered that the black specks are substantially, if notcompletely water-insoluble as measured at room temperature, (20-25° C.).A chemical analysis of these specks reveals that they compriseoligomeric/polymeric tannoids having no aromatic hydrogen.

We have also determined that the black specks have a particle size of onthe order of about 20μ down to 1 micron Thus, it has been observed thatsome black specks pass through a 5 micron filter but hardly any passthrough a one micron filter.

Without being bound by an explanation of the cause of the black specks,it is believed that the black specks are oxidation products, likely ofphenolic hydroxy groups and/or oligomeric or polymeric tanninsespecially those having a molecular weight of above on the order of3000.

We have discovered that such black specks and also oligomeric andpolymeric tannins are substantially, if not completely water-insoluble,and that they are biologically inactive materials.

Thus, another aspect of this invention is to provide at least twoprocesses which will remove the water-insoluble oligomeric and polymerictannins, especially such tannins having a molecular weight of over 1000.preferably over 2000 and particularly over 3000 (hereinafter referred toas polymeric tannins). By water-insoluble it meant that a 1% by weightconcentration of polymeric tannin in water does not exhibit a solubilityof more that 10% by weight of the total tannin at 22° C.

Still another aspect is to provide substantially water-soluble (over 95%by weight) extracts of Phyllanthus Emblica comprising, for example, lessthan 5% by weight of polymeric tannins, with substantially no blackspecks and at high levels, e.g. over 70% by weight of bio-active, lowmolecular-weight hydrolysable tannins having molecular weights below1,000. The resultant extracts can be used for all applicationspreviously described in the prior art: e.g. in cosmetic formulations,for example, skin lightening or even-toning, anti-aging and sunscreens,as well as in nutritional supplements and any new applications developedin the future.

A powdered composition of Emblica officinalis wherein said compositionis macroscopically substantially to completely devoid of black specks isa further embodiment of this invention.

A powdered composition of Emblica officinalis, wherein such compositioncontains at least 70% by weight of bio-active low molecular weighthydrolysable tannins is a further embodiment of this invention.

A powdered composition of Emblica officinalis, wherein the compositioncontains less than 5% by weight of oligomeric and polymeric tanninshaving a molecular weight of above 1000, preferably less than 5% byweight of oligomeric and polymeric tannins having a molecular weight ofabove 2000, and especially preferred less than 5% by weight ofoligomeric and polymeric tannins having a molecular weight of above 3000is a further embodiment of this invention.

The powdered compositions of Emblica officinalis can preferably compriseone or more water soluble diluents, preferably selected from the groupcomprising lactose, mannitol, dextrates, maltodextrin, dextrin,dextrose, and sucrose. The diluents are preferably present in an amountof 10 to 60% by weight.

Upon further study of the specification and dependent claims, furtheraspects and advantages of the inventions will become apparent.

To attain the objectives of the invention, there is provided at leastone process which comprises preventing the formation of black specksand/or precursors thereof and/or polymeric tannins. Also provided is atleast one process for separating the black specks and/or precursorsthereof and/or the polymeric tannins from the remainder of thecomponents of extracts of Emblica officinalis.

In general, the invention process comprises the following steps:

1) Providing an extract of Emblica officinalis either resulting from theoriginal extract from the plant, or from a suspension of a powderedcomposition obtained after the extract is processed, e.g. after a dryingstep.

2) If necessary, physically separating the black specks and/orprecursors thereof and/or polymeric tannins from the water-solublecomponents, for example by filtration with the use of a filter aid.

3) If desired, concentrating the resultant aqueous solution of theenriched composition of Emblica officinalis, for example to a drypowder.

With respect to step (1), if it is to be subjected to step (2), it ispreferred to mix the raw extract or powdered extract with an aqueoussolution preferably water. (By aqueous solution is meant water ormixture of water and a miscible solvent.) It is further preferred thatthe suspension contain about 5-30% more preferably about 18-22% byweight of total solids (including both dissolved and non-dissolvedsolids), and more preferably about 18-22%. When the extract is obtainedfrom the fruit, the extraction is preferably conducted, under conditionsso as to substantially prevent formation of polymeric tannins, e.g. lowtemperature (about 20° C. to 60° C.) and/or preferably under asubstantially non-oxidizing atmosphere, e.g., the pressing apparatus iscontinuously flushed with nitrogen, and/or the addition of anautooxidation inhibitor, e.g. a saline solution. Likewise, the dryingstep is preferably conducted under conditions of temperature, time andatmosphere so as to mitigate the formation of black specks and/orpolymeric tannins, examples of such conditions including but limited todrying at low temperature (freeze drying), short residence times in thespray drier, for example up to about 1 minute) and drying under vacuumat temperatures below 50° C.

If step (1) is nevertheless conducted under such conditions as to formblack specks and/or precursors thereof, and/or polymeric tannins, it isnecessary to conduct step (2).

As for step (2), the preferred separation method will take into accountthe physical and/or chemical properties of the black specks and/orprecursors thereof. For example, as indicated above, in “EMBLICA”, theblack specks have a particle size of approximately, of about 20μ orless.

Ideally, it would be preferred to provide a method of separation whichretains the bio-active components of EMBLICA by removing only theundesired components. Whereas there are a variety of separationprocedures that can be employed, e.g. any one of a number of well-knownfiltration or centrifugation processes or combinations thereof, it isalso contemplated that still other separation processes can be employedsuch as, for example, sedimentation, flotation and elutriation. A filteraid, e.g. diatomite filter aids, cross-linked polyvinyl pyrrolidone aswell as silica and silicate sorbents can also be used to remove theoligomeric/polymeric materials. Some of the suppliers of these filteraids are Advanced Minerals (Celpure 25, 65 & 100, AW Cellite NF, MPHarborlite), International Specialty Products (Plasdone XL), UnitedPerlite Corporation (Ultralite Perlite 505, 606C, 606F, 808, 909C,909F). Likewise, extraction of the black specks or precursors thereofwith a substantially water-miscible solvent, e.g. (ethanol, methanol,isopropanol or mixture of solvents) is also contemplated. For furtherdetails of separation systems, reference is made to descriptions in thepatent and chemical engineering literature, for example, section 19(liquid-solid systems) in Perry's Chemical Engineer's Handbook, 6thedition, editors Perry, Green and Maloney, 1984, McGraw-Hill BookCompany.

With respect to step (3), a concentrated composition of water-solubleEMBLICA components can be produced by any number of conventionalchemical engineering drying techniques. e.g. those described in Section20 of Perry's Chemical Engineer's Handbook, 6th edition, and includingbut not limited to tray dryers, rotary dryers, agitated dryers, gravitydryers, vibrating-conveyor dryers, pneumatic conveyor dryers, Glattdryers, freeze dryers and spray dryers. It is contemplated that prior tothe drying step that the aqueous solution of the desired Emblicaoffinalis components can optionally be subjected to evaporation undersufficiently low temperatures so as to not to deleteriously affect thecomponents. In view of the nature of the components, it is contemplatedin order to forestall decomposition during drying that drying undervacuum, e.g.—freeze drying, will be preferred over a high temperaturespray drying technique.

Without intending to be bound by the chemical structure, thewater-insoluble oligomeric/polymeric components of Phyllanthus emblicaextract appear to be based on the following general structure ofmonomeric units:

wherein R represents OH or ═O; and C-2/C-3 can have an unsaturation.

The arrow heads indicate the points of substitution meaning a fullyaromatic-substituted product. The substituted moieties comprise othermonomeric units which can be attached via a C—C bond and/or a C—O bond.

As for the evidence of the above depicted structure, the 300 MHz ¹H-NMRspectrum of the acetylated product, in CDCl₃ showed complete absence ofAromatic H signals. It is important to note that theseoligomeric/polymeric tannins may create adverse health problems as theycan combine irreversibly with some proteins. Hence, their presence is tobe avoided.

One process to avoid the formation of oligomeric/polymeric tanninscomprises the introduction of a small amount of salt solution,preferably sodium or potassium chloride, during the processing of thefruit juice. This salt solution inhibits the facile autooxidation of thesmall gallo-ellagi tannins into oligomeric/polymeric tannins. Inaddition to sodium or potassium chloride, it is contemplated that theaddition of any non-reactive, soluble, ionizable compounds will increasethe ionic strength of the reaction solution and will therefore inhibitoligomerization/polymerization.

By substituting the enriched compositions of Emblica officinalisproduced by the present invention for the non-enriched Emblica extracts,substantial advantages are obtained. Examples of such compositionsinclude but are not limited to skin and personal care compositions, e.g.sunscreens, as well as pharmaceutical and nutritional compositions.

Without further elaboration, it is believed that one skilled in the art,can, using the preceding description, utilize the present invention toits fullest extent. The following embodiments are, therefore, to beconstrued as merely illustrative and not limitative of the remainder ofthe disclosure in any way whatsoever. (These embodiments have not beennecessarily actually conducted or prepared.)

EXAMPLES Example 1

A 20% by weight of an aqueous dispersion of EMBLICA powder was preparedby mixing the EMBLICA in water in a stainless-steel container with ahand-held agitator for about 15 minutes in order to obtain an uniformdispersion.

The properties of the EMBLICA powder, were as follows:

Low molecular weigh tannins −77.8% by HPLC

Water insoluble material −12.2%

Pale yellow powder

The resultant dispersion was then subjected to centrifugal filtrationusing a centrifuge (Heinkel HF 300, bowl diameter 300 mm, filter area0.1 m²). 3L of a 10% solution of EMBLICA were filtered at a centrifugespeed of 1500 rpm. The filtration was complete within 10 min and yieldedthe curve of weight filtration diplayed in FIG. 1. The filter clothporosity was 5 μm.

Filtered material was dried to a powder using a spray drier.

Example 2

Using the same centrifuge employed in Example 1, two tests wereperformed at a 33% by weight concentration of EMBLICA in purified waterbut with different centrifugation speeds, i.e. different g forcesapplied to the product. Two first tests of 3 L each were filtered at1500 rpm (˜375 g) and the liquid recovered. In a second step, 8 L werefiltered in several parts at 3000 rpm (˜1500 g) to determine if furtherliquid extraction can be achieved. A filter of 1 μm porosity (model 3 54FC) was chosen since it gave a reasonable liquid cross-flow. Also, thisis the same filter used in previous filtration test with a 20% solutionwhich gave good results. The EMBLICA used in these tests have samecharacteristics as described in Example 1.

Test 1

3 L of a 33% solution of EMBLICA were filtered at a centrifuge speed of1500 rpm. The filtration was slower than at 20% but almost completeafter 15 min. The resulting filtrate solution constituting about ⅔ byweight of the original solution was opaque and about 70% initialmaterial was recovered. In order to increase the recovery, a second testwas made a higher centrifugation speed. No black particles were visually(macroscopically) observed in the filtrate but many were observed on theresidue on the filter.

Test 2

33% EMBLICA solution was filtered by using the same filter but a highercentrifugation speed of 3000 rpm. Filtration was only slightly improveddespite a 4 times higher g force. Out of 12 kgs of initial material,only 8.3 kgs were obtained. No black particles were observed in thefiltrate solution. Accordingly, filtration tests with a 33% w/w solutionof EMBLICA show satisfactory elimination of black particles, similar toprevious tests with 10 and 20% solutions. However, 33% weightconcentration appears too high for maximal product throughput.Filtration at 18-22% is therefore preferred.

Example 3

The solutions of Example 2 obtained by filtration at 1500 and 3000 rpmwere spray dried separately. Conditions were an inlet temperature of345±5° F., an outlet temperature of 230±5° F. and a feed rate of 100ml/min. The spray drier was a 30 inch Bowen Lab unit.

The laboratory results were as follows:

Processed first:

3000 rpm solution INPUT: 8.2 kgs OUTPUT: 1.395 kgs (+1.2 kgs) followedby

1500 rpm solution INPUT: 3.7 kgs OUTPUT: 1.06 kgs (+0.37 kgs)

The OUTPUT weights correspond to the direct product obtained as well asthe weight of sticking product brushed off the vessel's walls. Thelatter product caused by hot steel walls of the vessel shows a clearlydarker color (orangish-brownish) than the direct dried product(off-white to light beige). To overcome such sticking it is contemplatedthat production vessels will include an additional insulation of thewalls which will reduce, if not eliminate, this effect. No significantloss of material occurs during the spray drying process. The resultingproduct powder is quite dry, fluffy and slightly whiter than theoriginal.

The highest product loss occurred during the centrifuge filtration stepdue to the high initial concentration in the test. A much higherfiltration throughput can be obtained by using a 20%/w. solution.

The following table provides a chromatographic analysis of 2 lots.

Emblica™ (Centrifuge-Spray Dried Sample): Calculation of Actives fromHPLC Data

${\%\quad{small}\quad{tannoids}} = \frac{\Sigma\quad{areas}\quad{of}\quad{active}\quad{peaks}}{{Total}\quad{area}\quad{of}\quad{the}\quad{chromatogram}}$Lot No. F15

Areas for the actives: Emblicanin A+EmblicaninB+Punigluconin+Pedunculagin=Areas of peaks 1, 3, 6,8=894.95+513.28+261.87+891.97=2,562.07 Total area per HPLC: 2,929.93

% of actives=2,562.07/2,929.93=87.45%

% of Emblicanin A=894.95/2,929.93=30.55%

% of Emblicanin B=513.28/2,929.93=17.52%

% of Punigluconon=261.87/2,929.93=8.95%

% of Pedunculagin=891.97/2,929.93×83.80=30.44%

Lot No. F30

Areas for the actives: Emblicanin A+EmblicananB+Punigluconin+Pedunculagin+Areas of peaks 1, 3, 6,8=904.51+502.66+251.66+889.70=2,548.53

Total area per HPLC: 2,995.03

% of actives=2,548.53/2,995.03=85.10%

% of Emblicanin A=904.51/2,995.03=30.20%

% of Emblicanin B=502.66/2,995.03=16.79%

% of Punigluconon=251.66/2,995.03=8.40%

% of Pedunculagin=889.70/2,995.03=29.70%

Example 4

A 20% by weight of an aqueous dispersion of EMBLICA powder (100 Kg) wasprepared by mixing the EMBLICA in water in a stainless-steel vesselfilled with a mechanical agitator for about 1 hr in order to obtain anuniform dispersion. Then about 5 Kg of a diatomite filter aid (Celpure1,000) was blended well to bind oligomeric/polymeric tannins. The slurrywas mixed for approximately 30 min at room temperature. The residue wasremoved by centrifugation (i.e., in a Beckman™ J6B swinging one literbucket rotor at 3000 rpm for 5 min), or by pressure filtering (i.e.,through a coarse cellulose Cuno™. CPX-01A depth filter pad, with apressure of 5 psi, 35 kPa). The filtered aqueous solution was then driedeither by using a freeze drier or a spray drier.

Example 5

A 15% by weight of an aqueous dispersion of EMBLICA powder (10 Kg) wasprepared by mixing the EMBLICA in water in a stainless-steel vesselfilled with a mechanical agitator for about 1 hr in order to obtain auniform dispersion. Slight heating to about 30 to 40 C can expedite theprocess of dispersion. Then about 0.5 to 1 Kg of a diatomite filter aid(Celpure 1,000) was blended well to bind oligomeric/polymeric tannins.The slurry was mixed for approximately 30 min at room temperature andwas allowed to stay for about 5 to 10 hrs. Almost clear liquid on thetop was siphoned-off and then passed through a coarse filtration (cheesecloth) to remove any undesirable insoluble particulates. The aqueoussolution was then dried either by using a freeze drier or a vacuum drier(at about 55-60 C).

Example 6

The Emblica antioxidant fraction is obtained directly from the fruits byfollowing a three-step process: (1) Extraction: Emblica officinalisfruits were extracted with water or by squeezing the fruit flesh. (2)Removal of water-insoluble material: The fresh water-extract or thejuice was then subjected to centrifugation and the supernatant issiphoned-off. Alternately, the water extract or the juice was admixedwith a filter-aid and then filtered to remove the water-insolublematerial. (3) Drying: The water-soluble fraction was then dried undervacuum or freeze dried.

HPLC analysis showed that the powder of Emblica antioxidant fractioncontains 74.3% low molecular-weight hydrolysable tannins, the keybioactive components of the invention.

Example 7 Skin Care Lotion

TRADE INCI NAME NAME/MANUFACTURER % w/w Phase A Water (demineralized)65.97 Disodium EDTA 0.10 Propylene Glycol 2.00 Sorbitol Sorbo (70%soln.)/Uniqema 2.00 Sodium Lauryl Sulfate Stepanol ME-Dry/Stepan 0.15Phase B Glyceryl stearate Tegin M/Goldschmidt 5.00 Stearic acid Emersol132/Cognis 1.00 Persea Gratissima (Avocado) Crodarom Avocadin/Croda15.00 oil Unsaponifiables Beeswax White Bleached NF Beeswax 1.50Prills/Ross Phase C Water (demineralized) 5.00 Phyllanthus emblica fruitextract Present Invention* 1.00 Phase D Triethanolamine TEA 99%/UnionCarbide 0.28 Phase E Propylene glycol, DMDM Paragon/Mc Intyre 1.00Hydantoin, Methylparaben Total 100.00Procedure: Combine A and heat to 70-75° C. Combine B and heat to 70-75°C. Add B to A while stirring. Add phase C at 30° C. Adjust pH to 5.0-6.0with phase D. Add phase E. Mix until uniform.*By “Present Invention” is meant the enriched EMBLICA having a decreasedconcentration of black specks and oligomer/polymers.

Example 8 Skin Lightening Lotion

TRADE INCI NAME NAME/MANUFACTURER % w/w Phase A-1 Water (demineralized)56.18 Disodium EDTA 0.05 Propylene Glycol 5.00 Phase A-2 Xantham GumVanzan NF/Vanderbilt 0.25 Magnesium aluminum stearate Veegum Ultra 0.40granules/Vanderbilt Phase B Cetearyl alcohol and cetearyl Montanov68/Seppic 7.00 glucoside Apricot kernel oil Lipovol P/Lipo 10.00 Octylstearate Cetiol 868/Cognis 3.00 Dimethicone Dow Corning 200 Fluid 6.0010 cst/Dow Corning Phase C Water (demineralized) 10.00 Phyllanthusemblica fruit extract Present Invention 1.00 Phase D Triethanolamine TEA99%/Union Carbide 0.12 Phase E Phenoxyethanol, Liquapar PE/Sutton 1.00Isopropylparaben, Isobutylparaben, Butylparaben Total 100.00Procedure: Disperse A-2 in A-1 and heat to 70-75° C. Combine B and heatto 70-75° C. Add B to A while stirring. Homogenize until mixture coolsto 60° C. At 30° C. add phase C. Adjust pH with TEA to 4.0-5.0. Addphase E. Mix until uniform.

Example 9 Skin Lightening Lotion

TRADE INCI NAME NAME/MANUFACTURER % w/w Phase A-1 Water (demineralized)55.05 Disodium EDTA 0.05 Propylene Glycol 5.00 Phase A-2 Xantham GumVanzan NF/Vanderbilt 0.25 Magnesium aluminum stearate Veegum Ultra 0.40granules/Vanderbilt Phase B Cetearyl alcohol and cetearyl Montanov68/Seppic 7.00 glucoside Apricot kernel oil Lipovol P/Lipo 10.00 Octylstearate Cetiol 868/Cognis 3.00 Dimethicone Dow Corning 200 Fluid 6.0010 cst/Dow Corning Phase C Water (demineralized) 10.00 Phyllanthusemblica fruit extract Present Invention 2.00 Phase D Triethanolamine TEA99%/Union Carbide 0.25 Phase E Phenoxyethanol, Liquapar PE/Sutton 1.00Isopropylparaben, Isobutylparaben, Butylparaben Total 100.00Procedure: Disperse A-2 in A-1 and heat to 70-75° C. Combine B and heatto 70-75° C. Add B to A while stirring. Homogenize until mixture coolsto 60° C. At 30° C. add phase C. Adjust pH with TEA to 4.0-5.0. Addphase E. Mix until uniform.

Example 10 Age-Defying Lotion

TRADE INCI NAME NAME/MANUFACTURER % w/w Phase A-1 Water (demineralized)59.15 Disodium EDTA 0.05 Propylene Glycol 5.00 Phase A-2 Xantham GumVanzan NF/Vanderbilt 0.20 Phase B PEG-6 stearate, ceteth-20, Tefose2561/Gattefosse 10.00 glyceryl stearate, steareth-20, stearic acidStearic Acid Emersol 132/Cognis 1.00 Hydrogenated castor oil CutinaHR/Cognis 1.00 Octyldodecyl myristate M.O.D./Gattefosse 8.00 DimethiconeDow Corning 200, 50 4.00 cst/Dow Corning Phenyltrimethicone Dow Corning556 Wax/Dow 2.00 Coning Sweet Almond oil Cropure Almond/Croda 3.00 PhaseC Water (demineralized) 5.00 Phyllanthus emblica fruit extract PresentInvention 0.50 Phase D Triethanolamine TEA 99%/Union Carbide 0.10 PhaseE Phenoxyethanol, Liquapar PE/Sutton 1.00 Isopropylparaben,Isobutylparaben, Butylparaben Total 100.00Procedure: Disperse A-2 in A-1 and heat to 70-75° C. Combine B and heatto 70-75° C. Add B to A while stirring. Homogenize until mixture coolsto 60° C. At 30° C. add phase C. Adjust pH with TEA to 5.0-6.0. Addphase E. Mix until uniform.

Example 11 Sunscreen Lotion

TRADE INCI NAME NAME/MANUFACTURER % w/w Phase AButylmethoxydibenzoylmethane Eusolex 9020/Rona 1.00 Glyceryl Stearate,Ceteareth-15 Tegocare 215, Pellets/Degussa 3.00 Decyl oleate CetiolV/Cognis 5.00 Isopropyl palmitate Isopropyl palmitate 5.00 DimethiconeMlrasil DM 350 0.50 Stearyl alcohol Lanette 18 2.00 Carbomer CarbopolETD 2050 0.10 Phase B Glycerin Glycerol (about 87%) 3.00 Ectoin RonaCareEctoin/Rona 0.50 Phenoxyethanol, Liquapar PE/Sutton 1.00Isopropylparaben, Isobutylparaben, Butylparaben Aqua (water), Ethyhexyl15.00 metoxycinnamte, Silica, PVP, Chlorphenesin, BHT Water,demineralized Aqua (water) qs Phase C Phyllanthus emblica fruit extractPresent Invention 0.50 Phase D Sodium hydroxide Sodium hydroxide, 10%0.45 solution Phase E Perfume Fragrance delicat/Drom 0.20 Total 100.00Procedure: Heat phases A and B separately to 80 C. stir phase A.Homogenize. At 30 C, add phase C. Adjust pH with sodium hydroxide to5.5. Finally add phase E to the emulsion.

Example 12 Anhydrous Oil-Free Gel

TRADE INCI NAME NAME/MANUFACTURER % w/w Phase A Ozokerite WhiteOzokerite SP-1020/Strahl & 3.00 Pitsch Cyclomethicone Dow Corning 345Fluid/Dow 25.00 Corning Cyclomethicone (and) Gransil GCM/GrantIndustries 60.00 Polysilicone-11 Phase B Bismuth Oxychloride Biron ®LF-2000/Rona 2.00 Phase C Cyclomethicone Dow Corning 345 Fluid/Dow 3.60Corning Cyclomethicone (and) Dow Corning 9040 Silicone 5.40 DimethiconeCrosspolymer Elastomer Blend/Dow Corning Present Invention 1.00 Total100.00Procedure: Blend ingredients in Phase A; heat with mixing until clearand uniform. Add bismuth oxychoride and disperse with mixing. Blendingredients in Phase C separately; the mixture should be smooth andcontain no lumps. Cool Phase A/B to 50-60° C. and add Phase C withmixing. When the mixture is uniform it may be packaged.

Example 13 Capsules & Tablets

Procedure: 1 is granulated with starch paste to make it a free flowingpowder. Blend all the ingredients, except 4, for 25 min. in a blender.Screen in 4 and blend for an additional 5 min. Compress into tabletsusing 7/16 in standard concave tooling. Alternately, the blendedmaterial can be filled into appropriate capsules.

Example-14 Tablets and Capsules

Composition Quantity per Ingredient (w/w, in %) tablet (mg) 1. InventiveComposition 60.0 250.0 2. Avicel pH 101 20.0 84.0 3. Starch 1500 or 17.575.5    Maltodextrin 4. Steric acid, N.F. (powder) 2.0 8.5 5. Cab-O-Sil0.5 2.0Note:Emblica officinalis water soluble extract is granulated with starchpaste or maltodextrin to make it a free-flowing powder.

Procedure: Blend all the ingredients, except 4, for 25 min. in ablender. Screen in 4 and blend for an additional 5 min. Compress intotablets using 7/16 in standard concave tooling. Alternately, the blendedmaterial can be filled into appropriate capsules.

Example 15 Chewable Tablets

Composition Quantity per Ingredient (w/w, in %) tablet (mg) 1. InventiveComposition 9.26 26.60 2. Sodium ascorbate, USP 36.26 81.60 3. Avicel pH101 19.12 38.50 4. Sodium saccharin, (powder), N.F. 0.56 1.25 5. DiPac29.30 66.00 6. Stearic acid, N.F. 2.50 5.60 7. Imitation orange Flavor1.0 2.25 8. FD & C Yellow #6 dye 0.5 1.12 9. Cab-O-Sil 0.5 1.12

Procedure: Blend all the ingredients, except 6, for 20 min in a blender.Screen in 6 and blend for an additional 5 min. Compress into tabletsusing 7/16-in standard concave tooling.

Example 16 Beverages

Ingredient Quantity per 500 ml 1 Present Invention 10 mg-2 gm 2Excipients: Carbonated Water, Food Starch-q.s, Modified, High FructoseCorn Syrup and/or Sucrose and/or Sugar, Sodium Benzoate, Caffeine,Glycerol Ester of Wood resin, Flavors, Colors

Example 17 Cereals

Ingredient Quantity per 1 Kg 1. Extract of Invention 500 mg-10 gm 2.Excipients: Whole Grain Oats, Oat Bran, q.s, Sugar, Modified CornStarch, Brown Sugar Syrup, Salt, Calcium Carbonate, Trisodium Phosphate,Wheat Flour, Vitamin E (Mixed tocopherols), Zinc & Iron Mineralnutrients), Niacinamide (A B Vitamins), Vitamin B6 (Pyridoxine HCl),Vitamin B2 Riboflavin), Vitamin B1 (Thiamin Mononitrate), Vitamin A(Palmitate), Vitamin A B (Folic acid), Vitamin B12, Vitamin D

Example 18 Maintenance Multivitamin Tablets and Capsules

Composition Quantity per Ingredient (w/w, in %) tablet (mg) 1. Vitamin Aacetate 5.5 11.0 2. Thiamine mono-nitrate, USP 0.8 1.65 3. Riboflavin,USP 1.1 2.10 4. Pyridoxine HCl, USP 1.0 2.10 5. 1% Cyanocobalamine (ingelatin) 1.0 2.10 6. D-Calcium pantothenate, USP 3.75 7.50 7. InventiveComposition, free-flowing 32.25 65.50 8. Niacinamide 11.0 22.00 9. DiTab13.1 26.20 10. Microcrystalline cellulose, N.F. 25.0 50.00 11. Talc, USP3.0 6.00 12. Stearic acid, (powder), N.F. 1.5 3.00 13. Magnesiumstearate, (powder), N.F. 1.0 2.00

Procedure: Blend all ingredients for 20 min in a suitable blender.Screen in 12 and blend for an additional 5 min. Compress at a tabletweight of 200 mg using ⅜-in standard concave tooling. Alternately,blended material is filled into a capsule containing 200 mg ofmulti-vitamins. These tablets or capsules can be used as nutritionalsupplements.

Notwithstanding the details of the preceding embodiments, it is to beunderstood there are several broad concepts in the present invention.

The first broad concept relates to the treatment of a raw extract fromEmblica officinalis. Once it is known that it is important to adjust thetime, and/or temperature, and/or atmosphere and/or chemistry of theconditions of the extraction as to inhibit the formation of polymerictannins and/or black specks, a chemical engineer or the like would beable to adjust such variables so as to inhibit the formation of theundesired components. This would require measuring the extent of theundesired components without adjustment of the variables and thenadjusting the variables so as to provide an improved process. Forexample, lower temperatures and shorter residence times should result ina lower degree of oligomerization or polymerization. Likewise, the lessoxygen in the atmosphere, the less likelihood of oxidation to formundesired impurities. Consequently, by adjusting at least one of thevariables, it is possible that only one variable need be adjusted inorder to obtain the desired inhibition, for example, temperature.Nevertheless, it is also contemplated that two or more variables mayalso be adjusted so as to arrive at the optimum conditions.

Another basic concept of the invention relates to concentrating theextract, e.g. in order to form a powder. Again, the temperature, timeand atmosphere in which the concentrating is conducted will have aneffect on the degree of impurities in the resultant dried composition.Consequently, a chemical engineer or the like will be able to adjust atleast one of the variables in order to obtain a product which issubstantially to completely devoid of black particles when viewedvisually (macroscopically), preferably at least 95%, more preferably atleast 99%). By “substantially devoid” is meant that the black particlesare decreased in number compared to the number of black particles whichwould be present in the absence of the adjustment of the variables.Preferably, the composition should be completely devoid of black specks)but it is contemplated that it would be sufficient for esthetic purposesfor the composition to contain not more than 100, preferably below 10black specks per 500 grams of composition).

Another concept of the invention relates to the reduction of potentiallybiologically adverse components in the extract. This is accomplished,for example, by removing at least a portion of polymeric tannins havinga molecular weight of above 1,000, and especially above 3000.

Thus, taking into consideration the various concepts and aspects of theinvention, the preceding examples can be repeated with substantiallysimilar success by substituting generically or specifically describedsteps and/or operating conditions for those set forth in the examples.

The entire disclosure of all applications, patents, and publicationscited above, including those references set forth in said applications,patents and publications are hereby incorporated by reference.

From the foregoing description, one skilled in the art can easilyascertain the essential characteristics of this invention and withoutdeparting from the spirit and scope thereof, can make various changesand modifications of the invention to adapt it to various usages andconditions.

Short Explanation of the Figures

FIG. 1: Curve of weight filtration obtained according to Example 1

1. Extraction process comprising extracting a raw extract from Emblicaofficinalis wherein the extraction is conducted under conditions oftime, temperature and atmosphere, to inhibit the formation of blackspecks and/or oligomeric and/or polymeric tannins and/or oxidationproducts thereof.
 2. A process according to claim 1, comprisinginhibiting the formation of said oilgomeric and/or polymeric tanninshaving a molecular weight above
 1000. 3. Process of producing a powderedextract of Emblica officinalis, comprising the step of drying an aqueoussolution of the extract, wherein the drying is conducted underconditions of time, temperature and atmosphere so as to inhibit theformation of oligomeric and/or polymeric tannins and/or oxidationproducts thereof and/or black specks.
 4. A process according to claim 3comprising inhibiting the formation of said oligomeric and/or polymerictannins having a molecular weight above
 1000. 5. A process comprisingenriching an extract of Emblica officinalis, comprising the steps of: A)providing an aqueous suspension of Emblica officinalis, said aqueoussuspension containing dissolved components of Emblica officinalis andwater-insoluble components comprising black specks and/or oligomeric andpolymeric tannins; and B) separating the insoluble components from saiddissolved components to obtain an enriched aqueous extract of Emblicaofficinalis.
 6. A process according to claim 5, further comprising apreceding step of dispersing a powdered extract of Emblica officinalisin an aqueous solution to form said aqueous suspension.
 7. A processaccording to claim 5, wherein said separating comprises subjecting saidsuspension to centrifugation or pressure filtration.
 8. A processaccording to claim 5, wherein said separating comprises adding afilter-aid to said aqueous suspension and filtering out the insolublecomponents of the suspension so as to obtain an enriched aqueousfiltrate of Emblica officinalis.
 9. A process according to claim 5,wherein said aqueous suspension has a concentration of 5-30% by weight,preferably 18-22% by weight of total solids of Emblica officinalis. 10.A process according to claim 5, comprising subjecting said aqueoussuspension to sufficient centrifugation to obtain an enriched extract ofEmblica officinalis macroscopically substantially to completely devoidof black specks.
 11. A process according to claim 5, further comprisingdrying the separated enriched aqueous extract of Emblica officinalis.12. A process according to claim 5, wherein said drying step comprisesspray drying or freeze drying.
 13. A process according to claim 5,comprising drying said solution of Emblica officinalis under conditionsof time, temperature and atmosphere so as to inhibit the formation ofoligomeric and/or polymeric tannins having a molecular weight of over1000.
 14. An extract of Emblica officinalis produced by the process ofclaim 1
 15. Powdered composition of Emblica officinalis, the improvementwherein said composition is macroscopically substantially to completelydevoid of black specks.
 16. Powdered composition of Emblica officinalis,wherein such composition contains at least 70% by weight of bio-activelow molecular weight hydrolysable tannins.
 17. Powdered composition ofEmblica officinalis, wherein the composition contains less than 5% byweight of oligomeric and polymeric tannins having a molecular weight ofabove 1000, preferably less than 5% by weight of oligomeric andpolymeric tannins having a molecular weight of above 2000, andespecially preferred less than 5% by weight of oligomeric and polymerictannins having a molecular weight of above
 3000. 18. Powderedcomposition of Emblica officinalis according to claim 15, characterizedin that the composition comprises one or more water soluble diluents,preferably selected from the group comprising lactose, mannitol,dextrates, maltodextrin, dextrin, dextrose, and sucrose, wherein thediluents are preferably present in an amount of 10 to 60% by weight. 19.A skin or hair or personal care composition formed from ingredientscomprising a powdered composition according to claim
 15. 20. A skin orpersonal care composition according to claim 19 in the form of a lotion,creme, stick, spry or gel.
 21. A skin or personal care compositionaccording to claim 19 which contains about 0.05 to 5% of said tannins.22. A pharmaceutical or nutritional composition formed from ingredientscomprising a powdered composition according to claim 15 in the form of atablet, capsules, elixir, syrup, or drinks.
 23. A pharmaceutical ornutritional composition according to claim 22 formed from about 0.05 to20% of said powdered composition.